Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts

Autores
Ocsachoque, Marco Antonio; Eugenio Russman, Juan I.; Irigoyen, Beatriz del Luján; Gazzoli, Delia; Gónzalez, María Gloria
Año de publicación
2016
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Sulfur deactivation of Ni/CeO2 and Rh/CeO2 catalysts were examined through an experimental and theoretical study. These catalysts were characterized by N2 adsorption, X-ray diffraction, temperature programmed reaction, thermogravimetric analysis, Uv-visible spectroscopy and Raman spectroscopy, and tested under the methane dry reforming reaction in the presence of H2S. On the other hand, different possible interactions of sulfur with Rh, Ni or surface sites of the CeO2 support were evaluated by performing energy calculations with the density functional theory (DFT). Overall, the results indicate that tolerance to sulfur of Rh/CeO2 catalyst is higher than that of Ni/CeO2 one. In this sense, TPR measurements show that reduction of CeO2 is promoted by the presence of Rh. This effect, probably caused by hydrogen spillover to CeO2 support during the reduction of RhOx species, could be linked to a high oxygen donation capacity of Rh/CeO2 catalysts. Accordingly, the O2- species existing on Rh/CeO2 catalysts, revealed by Raman spectra of these samples, could favor sulfur oxidation and prevent Rh-S interactions. Likewise, the theoretical calculations show that desorption of S-O species from Rh/CeO2 system is more favorable than that from Ni/CeO2 one. Therefore, our experimental and theoretical study about sulfur deactivation of Ni and Rh supported on CeO2 allow us to postulate that Rh can help to desorb SOx species formed on the support, retarding sulfur poisoning of the Rh/CeO2 catalysts.
Fil: Ocsachoque, Marco Antonio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas "Dr. Jorge J. Ronco". Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Centro de Investigación y Desarrollo en Ciencias Aplicadas; Argentina
Fil: Eugenio Russman, Juan I.. Universidad de Buenos Aires. Facultad de Ingeniería. Departamento de Ingeniería Química; Argentina
Fil: Irigoyen, Beatriz del Luján. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; Argentina
Fil: Gazzoli, Delia. Instituto de Investigaciones Universitarias Roma la Sapienza; Italia
Fil: Gónzalez, María Gloria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas "Dr. Jorge J. Ronco". Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Centro de Investigación y Desarrollo en Ciencias Aplicadas; Argentina
Materia
Computer Modeling And Simulation
Oxides
Raman Spectroscopy And Scattering
Surface Properties
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/40025
Acceder
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network_name_str CONICET Digital (CONICET)
spelling Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalystsOcsachoque, Marco AntonioEugenio Russman, Juan I.Irigoyen, Beatriz del LujánGazzoli, DeliaGónzalez, María GloriaComputer Modeling And SimulationOxidesRaman Spectroscopy And ScatteringSurface Propertieshttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2Sulfur deactivation of Ni/CeO2 and Rh/CeO2 catalysts were examined through an experimental and theoretical study. These catalysts were characterized by N2 adsorption, X-ray diffraction, temperature programmed reaction, thermogravimetric analysis, Uv-visible spectroscopy and Raman spectroscopy, and tested under the methane dry reforming reaction in the presence of H2S. On the other hand, different possible interactions of sulfur with Rh, Ni or surface sites of the CeO2 support were evaluated by performing energy calculations with the density functional theory (DFT). Overall, the results indicate that tolerance to sulfur of Rh/CeO2 catalyst is higher than that of Ni/CeO2 one. In this sense, TPR measurements show that reduction of CeO2 is promoted by the presence of Rh. This effect, probably caused by hydrogen spillover to CeO2 support during the reduction of RhOx species, could be linked to a high oxygen donation capacity of Rh/CeO2 catalysts. Accordingly, the O2- species existing on Rh/CeO2 catalysts, revealed by Raman spectra of these samples, could favor sulfur oxidation and prevent Rh-S interactions. Likewise, the theoretical calculations show that desorption of S-O species from Rh/CeO2 system is more favorable than that from Ni/CeO2 one. Therefore, our experimental and theoretical study about sulfur deactivation of Ni and Rh supported on CeO2 allow us to postulate that Rh can help to desorb SOx species formed on the support, retarding sulfur poisoning of the Rh/CeO2 catalysts.Fil: Ocsachoque, Marco Antonio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas "Dr. Jorge J. Ronco". Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Centro de Investigación y Desarrollo en Ciencias Aplicadas; ArgentinaFil: Eugenio Russman, Juan I.. Universidad de Buenos Aires. Facultad de Ingeniería. Departamento de Ingeniería Química; ArgentinaFil: Irigoyen, Beatriz del Luján. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; ArgentinaFil: Gazzoli, Delia. Instituto de Investigaciones Universitarias Roma la Sapienza; ItaliaFil: Gónzalez, María Gloria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas "Dr. Jorge J. Ronco". Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Centro de Investigación y Desarrollo en Ciencias Aplicadas; ArgentinaElsevier Science Sa2016-04info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/40025Ocsachoque, Marco Antonio; Eugenio Russman, Juan I.; Irigoyen, Beatriz del Luján; Gazzoli, Delia; Gónzalez, María Gloria; Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts; Elsevier Science Sa; Materials Chemistry and Physics; 172; 4-2016; 69-760254-0584CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.matchemphys.2015.12.062info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0254058415305381info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:19:57Zoai:ri.conicet.gov.ar:11336/40025instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-10-22 11:19:57.635CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts
title Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts
spellingShingle Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts
Ocsachoque, Marco Antonio
Computer Modeling And Simulation
Oxides
Raman Spectroscopy And Scattering
Surface Properties
title_short Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts
title_full Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts
title_fullStr Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts
title_full_unstemmed Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts
title_sort Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts
dc.creator.none.fl_str_mv Ocsachoque, Marco Antonio
Eugenio Russman, Juan I.
Irigoyen, Beatriz del Luján
Gazzoli, Delia
Gónzalez, María Gloria
author Ocsachoque, Marco Antonio
author_facet Ocsachoque, Marco Antonio
Eugenio Russman, Juan I.
Irigoyen, Beatriz del Luján
Gazzoli, Delia
Gónzalez, María Gloria
author_role author
author2 Eugenio Russman, Juan I.
Irigoyen, Beatriz del Luján
Gazzoli, Delia
Gónzalez, María Gloria
author2_role author
author
author
author
dc.subject.none.fl_str_mv Computer Modeling And Simulation
Oxides
Raman Spectroscopy And Scattering
Surface Properties
topic Computer Modeling And Simulation
Oxides
Raman Spectroscopy And Scattering
Surface Properties
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv Sulfur deactivation of Ni/CeO2 and Rh/CeO2 catalysts were examined through an experimental and theoretical study. These catalysts were characterized by N2 adsorption, X-ray diffraction, temperature programmed reaction, thermogravimetric analysis, Uv-visible spectroscopy and Raman spectroscopy, and tested under the methane dry reforming reaction in the presence of H2S. On the other hand, different possible interactions of sulfur with Rh, Ni or surface sites of the CeO2 support were evaluated by performing energy calculations with the density functional theory (DFT). Overall, the results indicate that tolerance to sulfur of Rh/CeO2 catalyst is higher than that of Ni/CeO2 one. In this sense, TPR measurements show that reduction of CeO2 is promoted by the presence of Rh. This effect, probably caused by hydrogen spillover to CeO2 support during the reduction of RhOx species, could be linked to a high oxygen donation capacity of Rh/CeO2 catalysts. Accordingly, the O2- species existing on Rh/CeO2 catalysts, revealed by Raman spectra of these samples, could favor sulfur oxidation and prevent Rh-S interactions. Likewise, the theoretical calculations show that desorption of S-O species from Rh/CeO2 system is more favorable than that from Ni/CeO2 one. Therefore, our experimental and theoretical study about sulfur deactivation of Ni and Rh supported on CeO2 allow us to postulate that Rh can help to desorb SOx species formed on the support, retarding sulfur poisoning of the Rh/CeO2 catalysts.
Fil: Ocsachoque, Marco Antonio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas "Dr. Jorge J. Ronco". Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Centro de Investigación y Desarrollo en Ciencias Aplicadas; Argentina
Fil: Eugenio Russman, Juan I.. Universidad de Buenos Aires. Facultad de Ingeniería. Departamento de Ingeniería Química; Argentina
Fil: Irigoyen, Beatriz del Luján. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; Argentina
Fil: Gazzoli, Delia. Instituto de Investigaciones Universitarias Roma la Sapienza; Italia
Fil: Gónzalez, María Gloria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas "Dr. Jorge J. Ronco". Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Centro de Investigación y Desarrollo en Ciencias Aplicadas; Argentina
description Sulfur deactivation of Ni/CeO2 and Rh/CeO2 catalysts were examined through an experimental and theoretical study. These catalysts were characterized by N2 adsorption, X-ray diffraction, temperature programmed reaction, thermogravimetric analysis, Uv-visible spectroscopy and Raman spectroscopy, and tested under the methane dry reforming reaction in the presence of H2S. On the other hand, different possible interactions of sulfur with Rh, Ni or surface sites of the CeO2 support were evaluated by performing energy calculations with the density functional theory (DFT). Overall, the results indicate that tolerance to sulfur of Rh/CeO2 catalyst is higher than that of Ni/CeO2 one. In this sense, TPR measurements show that reduction of CeO2 is promoted by the presence of Rh. This effect, probably caused by hydrogen spillover to CeO2 support during the reduction of RhOx species, could be linked to a high oxygen donation capacity of Rh/CeO2 catalysts. Accordingly, the O2- species existing on Rh/CeO2 catalysts, revealed by Raman spectra of these samples, could favor sulfur oxidation and prevent Rh-S interactions. Likewise, the theoretical calculations show that desorption of S-O species from Rh/CeO2 system is more favorable than that from Ni/CeO2 one. Therefore, our experimental and theoretical study about sulfur deactivation of Ni and Rh supported on CeO2 allow us to postulate that Rh can help to desorb SOx species formed on the support, retarding sulfur poisoning of the Rh/CeO2 catalysts.
publishDate 2016
dc.date.none.fl_str_mv 2016-04
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/40025
Ocsachoque, Marco Antonio; Eugenio Russman, Juan I.; Irigoyen, Beatriz del Luján; Gazzoli, Delia; Gónzalez, María Gloria; Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts; Elsevier Science Sa; Materials Chemistry and Physics; 172; 4-2016; 69-76
0254-0584
CONICET Digital
CONICET
url http://hdl.handle.net/11336/40025
identifier_str_mv Ocsachoque, Marco Antonio; Eugenio Russman, Juan I.; Irigoyen, Beatriz del Luján; Gazzoli, Delia; Gónzalez, María Gloria; Experimental and theoretical study about sulfur deactivation of Ni/ CeO2 and Rh/CeO2 catalysts; Elsevier Science Sa; Materials Chemistry and Physics; 172; 4-2016; 69-76
0254-0584
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.matchemphys.2015.12.062
info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0254058415305381
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science Sa
publisher.none.fl_str_mv Elsevier Science Sa
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 12.982451

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